Fukuzawa, HironobuTakanashi, TsukasaKukk, EdwinMotomura, KojiWada, Shin-ichiNagaya, KiyonobuIto, YutaNishiyama, ToshiyukiNicolas, ChristopheKumagai, YoshiakiIablonskyi, DenysMondal, SubhenduTachibana, TetsuyaYou, DaehyunYamada, SyuheiSakakibara, YutaAsa, KazukiSato, YuhiroSakai, TsukasaMatsunami, KenjiUmemoto, TakayukiKariyazono, KangoKajimoto, ShinjiSotome, HikaruJohnsson, PerSchöffler, Markus S.Kastirke, GregorKooser, KunoLiu, Xiao-JingAsavei, TheodorNeagu, LiviuMolodtsov, SergueiOchiai, KoheiKanno, ManabuYamazaki, KaoruOwada, ShigekiOgawa, KanadeKatayama, TetsuoTogashi, TadashiTono, KensukeYabashi, MakinaGhosh, AryyaGokhberg, KirillCederbaum, Lorenz S.Kuleff, Alexander I.Fukumura, HiroshiKishimoto, NaokiRudenko, ArtemMiron, CatalinKono, HirohikoUeda, Kiyoshi2023-12-072023-12-072019-05-16https://hdl.handle.net/2097/44036The increasing availability of X-ray free-electron lasers (XFELs) has catalyzed the development of single-object structural determination and of structural dynamics tracking in real-time. Disentangling the molecular-level reactions triggered by the interaction with an XFEL pulse is a fundamental step towards developing such applications. Here we report real-time observations of XFEL-induced electronic decay via short-lived transient electronic states in the diiodomethane molecule, using a femtosecond near-infrared probe laser. We determine the lifetimes of the transient states populated during the XFEL-induced Auger cascades and find that multiply charged iodine ions are issued from short-lived (∼20 fs) transient states, whereas the singly charged ones originate from significantly longer-lived states (∼100 fs). We identify the mechanisms behind these different time scales: contrary to the short-lived transient states which relax by molecular Auger decay, the long-lived ones decay by an interatomic Coulombic decay between two iodine atoms, during the molecular fragmentation.Creative Commons Attribution 4.0 International Licensehttps://creativecommons.org/licenses/by/4.0/Text